EP0907970B1 - White light-emitting diode - Google Patents

White light-emitting diode Download PDF

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Publication number
EP0907970B1
EP0907970B1 EP98903213A EP98903213A EP0907970B1 EP 0907970 B1 EP0907970 B1 EP 0907970B1 EP 98903213 A EP98903213 A EP 98903213A EP 98903213 A EP98903213 A EP 98903213A EP 0907970 B1 EP0907970 B1 EP 0907970B1
Authority
EP
European Patent Office
Prior art keywords
light
nm
phosphor
emitting
phosphors
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired - Lifetime
Application number
EP98903213A
Other languages
German (de)
French (fr)
Other versions
EP0907970A1 (en
Inventor
Thomas JÜSTEL
Hans Nikol
Cees Ronda
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Philips Intellectual Property and Standards GmbH
Koninklijke Philips NV
Original Assignee
Philips Intellectual Property and Standards GmbH
Koninklijke Philips NV
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Priority to DE19708407 priority Critical
Priority to DE19708407 priority
Priority to DE1997156360 priority patent/DE19756360A1/en
Priority to DE19756360 priority
Application filed by Philips Intellectual Property and Standards GmbH, Koninklijke Philips NV filed Critical Philips Intellectual Property and Standards GmbH
Priority to PCT/IB1998/000219 priority patent/WO1998039805A1/en
Publication of EP0907970A1 publication Critical patent/EP0907970A1/en
Application granted granted Critical
Publication of EP0907970B1 publication Critical patent/EP0907970B1/en
Anticipated expiration legal-status Critical
Application status is Expired - Lifetime legal-status Critical

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    • HELECTRICITY
    • H01BASIC ELECTRIC ELEMENTS
    • H01LSEMICONDUCTOR DEVICES; ELECTRIC SOLID STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H01L33/00Semiconductor devices with at least one potential-jump barrier or surface barrier specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/48Semiconductor devices with at least one potential-jump barrier or surface barrier specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor body packages
    • H01L33/50Wavelength conversion elements
    • H01L33/501Wavelength conversion elements characterised by the materials, e.g. binder
    • H01L33/502Wavelength conversion materials
    • H01L33/504Elements with two or more wavelength conversion materials

Abstract

The invention relates to a light-emitting device comprising a UV diode with a primary emission of 300 nm ≤ μ ≤ 370 nm,and a phosphor layer consisting of a combination of a blue-light emitting phosphor with an emission band of 430 nm ≤ μ ≤ 490 nm, a green-light emitting phosphor with an emission band of 520 nm ≤ μ ≤ 570 nm and a red-light emitting phosphor with an emission band of 590 nm ≤ μ ≤ 630 nm, said device emitting high-quality white light. The colour rendering index CRI is 90 at a colour temperature of 4 000 K. As colour rendering depends only on the composition of the three phosphors and not on the relation of converted to non-converted light it is easyto control and regulate.

Description

  • The invention relates to a light emitting device for generating white light from a light emitting diode and a phosphor layer.
  • Light-emitting diodes are used as signal lamps, indicator displays, control and warning lamps, as light transmitters in photoelectric sensors, for optocouplers, IR remote control and optical fiber transmission systems. They offer a number of advantages over other light-emitting devices, e.g. Lightbulbs. They have a long service life, high shock and vibration resistance, good modulability up to the MHZ range, high packing densities, wide circuit compatibility and no inrush current peaks. They require a low operating voltage and have a low power consumption.
  • However, it has long been a drawback of the visible light emitting diodes that not all visible light colors with the same luminous intensity were available. The efficiency of the light-emitting diodes deteriorates with decreasing wavelength, i. from red to green to blue. While the brightness of red and green light-emitting diodes was very good and was considerably increased by modern production methods, blue light-emitting diodes had a relatively low light intensity. Therefore, it was not possible to achieve a color-neutral, white illumination by a combination of light-emitting diodes with simple means.
  • Theoretically, any color of visible light can be generated from shortwave light, ie, blue, violet, and ultraviolet light. It combines the light emitting diode, which emits short-wave light, with a suitable phosphor, which converts the short-wave light into the desired color, by absorbing the short-wave light and re-emitting light of the other color in the longer wavelength range.
  • White light can be z. B. with a blue emitting light emitting diode when combined with a phosphor which absorbs blue light, converts it and emits it as light in the yellow-orange region of the spectrum. The yellow-orange light mixes with the remaining portion of the blue light from the light-emitting diode and is obtained from blue together with the complementary color yellow white light.
  • For example, it is off JP 08007614 A (Patent Abstracts of Japan) discloses a planar light source using a light-emitting diode which emits blue light and which is combined with a fluorescent layer of an orange fluorescent pigment so that the blue light of the diode is observed as white light can. A disadvantage of this light source is that the hue of the white light is greatly affected by the small amount of the fluorescent pigment in the fluorescent layer and therefore difficult to control. Only with a high color temperature between 8000 and 8600 K, a good color rendering is obtained. If the color temperature is lowered, the color rendering index CRI also drops considerably.
  • Furthermore, it is off Jpn.J. Appl. Phys. Vol.35 (1996) pp. L838 - L839 a light source is known which has a blue light-emitting diode, which is also excited by a high injection current for the emission of UV light, and a phosphor mixture, the ZnS: Ag (blue), ZnS: Cu, Al (green) and ZnCdS: Ag ( red).
  • In the not pre-published WO 97/48138 is a lamp of an array of individual red, green, and blue phosphorous-converted UV LEDs that individually provide red green or blue light, or together provide white mixed light.
  • In addition, in EP 0446 846 Discloses dye preparations containing fluorescent europium complexes and their use in dye formulations for a thermal transfer color printing process.
  • It is the object of the present invention to provide a light-emitting device for producing white light, the color tone reproduction of which is easy to regulate and whose color rendering index is high.
  • According to the invention, the object is achieved by a light-emitting device with a UV diode having a primary emission of 300 nm ≦ λ≤370 nm and having a phosphor layer with a mixture of a blue-emitting phosphor having an emission band of 430 μm ≦ λ ≦ 490 nm, a green emitting phosphor which is a line emitter having an emission band having a maximum wavelength of 520 nm ≤ λ ≤ 570 nm and a red emitting phosphor which is a line emitter having an emission band having a wavelength maximum of 605 nm ≤ λ ≤ 620 nm.
  • The light-emitting device exhibits high color rendering and high efficiency at the same time because the phosphors absorb the UV band with high efficiency, the quantum efficiency is high - over 90% - and the half-width of the emission line is small. The light output is high because no light is emitted in the range above 440 nm and below 650 nm, where the eye sensitivity is low. -
  • The white light emitted from the light-emitting device is of high quality. The color rendering index CRI is 90 at a color temperature of 4000 K. The color rendering depends only on the composition of the three phosphors, not from the relation of converted to nonconverted light and is therefore easy to control and regulate.
  • In the context of the present invention it is preferred that the phosphors are lanthanide-activated phosphors, in particular that the phosphors are activated by Eu (III) or Tb (III).
  • It is also preferable that the blue-emitting phosphor is a line emitter having an emission band at 430nm ≦ λ ≦ 490nm.
  • It is further preferred that the UV diode is a GaN diode.
  • In the present invention, it may be preferable that the phosphor layer has a blue-emitting phosphor in an amount x1 of 0 <x1 ≦ 30 wt%, a green-emitting phosphor in an amount x2 of 20 ≦ x2 ≦ 50 wt. % and a red-emitting phosphor in an amount x3 of 30 ≦ x3 ≦ 70% by weight.
  • It may also be preferable that the phosphor layer contains BaMgAl 10 O 17 : Eu as the blue-emitting phosphor, ZnS: Cu as the green-emitting phosphor, and Y 2 O 2 S: Eu as the red-emitting phosphor.
  • In the context of the present invention it is particularly preferred that the phosphor layer has as red-emitting phosphor a phosphor of the composition [Eu (diketonate) a X b1 X ' b2 ], where X = pyridine or a monodentate pyridine derivative and X' = 2,2'- Bipyridine or a 2,2'-bipyridyl derivative and 2a + b 1 + 2b 2 = 8.
  • The invention will be further described with reference to a figure and three embodiments.
    • Fig. 1: light-emitting device
  • A light-emitting device according to the invention comprises a UV diode as excitation source for the UV radiation and a phosphor layer, with a mixture of three phosphors, which convert the UV light of the UV diode into visible, white light. In the embodiment shown in the drawing, the device is constructed so that the UV diode is embedded in a hemispherical cup of a polymer, which is arranged on a transparent substrate (front panel) 1 . The three phosphor powders 2 are finely distributed embedded in the polymer 3 . The polymer cup together with the phosphorus powder forms the phosphor layer. The device according to the invention may further comprise mirrors 4 for UV and visible light for improving the light extraction. For example, the cup itself may be formed as a reflector.
  • In the simplest case, the light-emitting device consists of a UV diode and a transparent coating applied thereto, which contains the phosphors. The transparent coating may, for example, contain the phosphors in a solid solution in a transparent matrix of polyacrylate, polystyrene, epoxy resin or another polymer.
  • As a mass product, LEDs are typically molded in epoxy resin housings, with a molded dome-shaped epoxy lens used to improve the extraction of light from the diode. In this embodiment, the phosphors can be applied as a contact layer between the actual diode and the epoxy resin dome. They can also be applied as a coating on the outside of the epoxy resin dome.
  • Large, two-dimensional, light-emitting devices can be easily manufactured by combining a diode array with the phosphor layer of the invention. For example, the diode array may be covered by a glass plate printed with the phosphors.
  • The UV diode is in particular a UV diode made of InGaN or GaN and has its emission maximum between 370 and 410 nm with a full width at half maximum FWHM < 50 nm.
  • To maintain the light emission means are provided for supplying electrical energy to the UV diode. These means comprise at least two electrodes.
  • The three phosphors are selected to be excited by the UV light of the UV diode and the red phosphorus has a narrow emission line at 590 mm ≤ λ ≤ 630 nm, the green phosphor a narrow emission line at 520 nm ≤ λ ≤ 570 nm and the blue phosphor has a narrow emission line at 430 nm ≦ λ ≦ 490 nm. For the blue phosphor, instead of a line emitter with a narrow emission line, a broadband emitter may also be used. The emission lines of the three phosphors can be tuned very precisely, even if the emissions are not completely independent of each other, as emission flanks partially overlap. This allows the color coordinates of the white light to be set accurately. The phosphors are preferably lanthanide-activated phosphors, for example Eu 3+ or Tb 3+ -activated phosphors.
  • As red phosphors are phosphors of the composition [Eu (diketonat) a X b1 X ' b2 ], wherein X = pyridine or a monodentate pyridine and X' = 2,2'-bipyridine or a 2,2'-Bipyridylderivat and 2a + b 1 + 2b 2 = 8, is preferred. These complex coordination compounds of europium (III) contain Eu 3+ as the metal center, diketonates as anionic chelate ligands and 2,2'-bipyridine or a 2,2'-bipyridyl derivative as neutral chelating ligands. As diketonates, pentane-2,4-dithionate (acac), 2,2,6,6-tetramethyl-3,5-heptanedithionate (thd), 1- (2-thenoyl) -4,4,4-trifluoro-1 , 3-butanedithionate (ttfa), 7,7-dimethyl-1,1,1,2,2,3,3-heptafluoro-4,6-octanedithionate (fod), 4,4,4-trifluoro-1- ( 2-naphthyl) -1,3-butanedithionate (tfnb), 1,3-diphenyl-1,3-propanedithionate (dbm), as the neutral ligands X pyridine, or the bidentate ligands 2,2'-bipyridine (bpy), 1 , 10-phenanthroline (phen), 4,7-diphenyl-1,10-phenanthroline (dpphene), 5-methyl-1,10-phenathroline (mphene), 4,7-dimethyl-1,10-phenanthroline (dimhene), 3,4,7,8-tetramethyl-1,10-phenanthroline (temphene), 5-nitro-1,10-phenanthroline (NOphen), 5-chloro-1,10-phenanthroline (Clphen) or dipyridinphenazine (dppz) ,
  • Table 1 shows blue-emitting, green-emitting and red-emitting phosphors with their wavelength maximum and their absorption at 370 nm. <B> Table. 1 </ b> Blue-emitting phosphors composition λ [max] Absorption at 370 nm [%] QE at 370 nm BaMgAl 10 O 17 : Eu 450 70 90 Sr 5 (PO 4 ) 3 Cl: Eu 450 70 90 ZnS: Ag 450 75 75 Green-emitting phosphors composition λ [max] Absorption at 370 nm [%] QE at 370 nm ZnS: Cu 550 40 85 BaMgAl 10 O 17 : Eu, Mn 515 70 90 Red emitting phosphors composition λ [max] Absorption at 370 nm [%] QE at 370 nm Y 2 O 2 S: Eu 3+ 628 30 90 YVO 4 : Eu 3+ 620 25 85 Y (V, P, B) O 4: Eu 3+ 615 25 85 YNbO 4 : Eu 3+ 615 20 90 YTaO 4 : Eu 3+ 615 20 90 [Eu (acac) 3 (phen)] 611 97 70
  • The mixture according to the invention gives a good color rendering index and at the same time a good energy yield. The light-emitting device has a color rendering index CRI <90 at a color temperature ≥4000 K and is thus suitable for interior lighting.
  • To produce the phosphor layer, the three phosphors can be applied as a coating with a binder on the diode surface. Suitable binders are, for example, film-forming acrylic polymers, such as methyl acrylate and polystyrene. Alternatively, they may be mixed in micrograms into the epoxy resin of the epoxy resin dome and evenly distributed throughout the epoxy resin dome. Instead of epoxy resin, another transparent thermoset can be used. This gives a more diffuse emission of white light. Because of the high brightness of the light emitting device, it may be desirable for security reasons that the light emission be more diffuse.
  • In operation, UV light having a wavelength λ ≦ 370 nm, which falls on the mixture of phosphors in the phosphor layer, is generated by the UV diode. These absorb the radiation and emit longer wavelength radiation, i. The phosphors transform the invisible UV radiation into visible light, which is converted by the phosphors into visible light. By mixing the three phosphors with different emission lines, the light of the desired composition is obtained.
  • Since the illumination of the light-emitting device according to the invention is not the light emitted by a glowing body but the excitation illumination of the phosphors in the phosphor layer, the luminous efficacy is extraordinarily high. The light-emitting device according to the invention provides a pleasant, true-to-life light. The visible emission lines of the phosphors are so close to each other that a quasi-continuous spectrum results, from which a good color rendition follows.
  • Embodiment 1
  • A light emitting device was made of a UV diode and a phosphor layer with a mixture of the three phosphors. An undoped GaN diode with transparent sapphire as the diode substrate was used. The diode substrate was coated with a suspension of three phosphors in various proportions as shown in Tab. 2 in a 1% polyvinyl alcohol solution and baked at 200 ° C. Tab. 2 T c [K] x 1 [BaMgAl 10 O 17 : Eu] x 2 [ZnS: Cu] x 3 [YVO 4 : Eu 3+ ] Ra8 Phosphor diode eff. [Lm / W] 2700 .04 .36 .60 85 9.7 3000 .08 .37 .56 85 9.8 4000 .16 .41 .43 91 9.9 5000 .22 .41 .36 92 9.6 6300 .28 .43 .30 96 9.8
  • Embodiment 2
  • A light emitting device was made of a UV diode and a phosphor layer with a mixture of the three phosphors. An undoped GaN diode with transparent sapphire as the diode substrate was used. The diode substrate was coated with a suspension of three phosphors in various proportions as shown in Tab. 2 in a 1% polyvinyl alcohol solution and baked at 200 ° C. Tab. 3 T c [K] x 1 [BAM] x 2 [ZnS: Cu] x 3 [Eu (acac) 3 (phen)] Ra8 Phosphor diode eff. [Lm / W] 2700 .06 .36 .54 82 12.0 3000 .1 .37 .49 83 11.9 4000 .18 .41 .37 89 11.8 5000 .25 .41 .31 91 11.4 6300 .30 .43 .25 95 11.3
  • Embodiment 3
  • A light emitting device was made of a UV diode and a phosphor layer with a mixture of the three phosphors. Has been used an undoped GaN diode with transparent sapphire as a diode substrate. The diode substrate was coated with a suspension of three phosphors in various proportions as shown in Tab. 2 in a 1% polyvinyl alcohol solution and baked at 200 ° C. Tab. 4 T c [K] x 1 [BAM] x 2 [ZnS: Cu] x 3 [Y 2 O 2 S: Eu 3+ ] Ra8 Phosphor diode eff. [Lm / W] 2700 12:05 12:31 0.63 85 12.2 3000 12:09 12:32 12:59 85 12.2 4000 12:16 12:38 12:46 89 12.7 5000 12:23 12:38 12:39 90 12.5 6300 12:28 12:40 12:32 95 12.5

Claims (8)

  1. A light-emitting device comprising an UV-diode with a primary emission of 300 nm ≤ λ ≤ 370 nm and a phosphor layer including a combination of a blue-emitting phosphor having an emission band at 430 nm ≤ λ ≤ 470 nm, a green-emitting phosphor being a line emitter having an emission band with a wavelength maximum of 520 nm ≤ λ < 570 nm, and a red-emitting phosphor being a line emitter having an emission band with a wavelength maximum of 605 nm ≤ λ ≤ 20 nm.
  2. A light-emitting device as claimed in claim 1, characterized in that the phosphors are lanthanide-activated phosphors.
  3. A light-emitting device as claimed in claim 2, characterized in that the phosphors are activated by Eu(III) or Tb(III).
  4. A light-emitting device as claimed in claim 1, characterized in that the blue-emitting phosphor is a line emitter having an emission band at 430 nm ≤ λ ≤ 490 nm.
  5. A light-emitting device as claimed in claim 1, characterized in that the UV-diode is a GaN diode.
  6. A light-emitting device as claimed in claim 1, characterized in that the phosphor layer comprises the blue-emitting phosphor in a quantity x1 of 0 < x1 ≤ 30% by weight, the green-emitting phosphor in a quantity x2 of 20 ≤ x2 ≤ 50% by weight and the red-emitting phosphor in a quantity x3 of 30 ≤ 3 ≤ 70% by weight.
  7. A light-emitting device as claimed in claim 1, characterized in that the phosphor layer comprises BaMgAl10O17:Eu as the blue-emitting phosphor, ZnS:Cu as the green-emitting phosphor and Y2O2S:Eu(III) as the red-emitting phosphor.
  8. A light-emitting device as claimed in claim 1, characterized in that the phosphor layer comprises as the red-emitting phosphor a phosphor of the composition [Eu(diketonate)aXb1X'b2], wherein X = pyridine or a monodentate pyridine derivative and X' = 2,2'-bipyridine or a 2,2'-bipyridyl derivative and 2a+b1+2b2 = 8.
EP98903213A 1997-03-03 1998-02-23 White light-emitting diode Expired - Lifetime EP0907970B1 (en)

Priority Applications (5)

Application Number Priority Date Filing Date Title
DE19708407 1997-03-03
DE19708407 1997-03-03
DE1997156360 DE19756360A1 (en) 1997-03-03 1997-12-18 white light-emitting diode
DE19756360 1997-12-18
PCT/IB1998/000219 WO1998039805A1 (en) 1997-03-03 1998-02-23 White light-emitting diode

Publications (2)

Publication Number Publication Date
EP0907970A1 EP0907970A1 (en) 1999-04-14
EP0907970B1 true EP0907970B1 (en) 2007-11-07

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US (1) US6084250A (en)
EP (1) EP0907970B1 (en)
JP (1) JP2000509912A (en)
DE (1) DE59814117D1 (en)
WO (1) WO1998039805A1 (en)

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US6084250A (en) 2000-07-04

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